Ni/PHAC催化甲醇羰基化合成乙酸工艺研究

Synthesis of Acetic Acid via Methanol Carbonylation Catalyzed by Nickels Supported on Phenolic-resine Derived Active Carbon

以自制的酚醛树脂基活性炭(PHAC)负载镍为催化剂、碘甲烷为助催化剂,研究了在连续固定床反应器中催化甲醇羰基化合成乙酸的反应。探讨了反应温度、液体进料空时、甲醇与一氧化碳配比及加水量等反应工艺条件对甲醇羰基化反应及乙酸收率的影响,优化了反应的工艺条件。结果表明:反应工艺条件对甲醇羰基化反应及乙酸的收率影响较大,在系统压力为1.0MPa,反应温度558K,液体进料空时为10gcat (mol h-1) -1, V(H2O):V(CH3OH)=3:100, n(CO):n(CH3OH):n(CH3I)=80:40:1的条件下乙酸收率最高达到了67.1%,而羰基化产物总收率可以达到79.1%,甲醇转化率可以达到93.8%,羰基化产物总收率和乙酸收率明显高于文献报道的同类催化剂。

The acetic acid was synthesized from methanol and carbon monoxide via carbonylation in fixed bed reaction. The self-made nickels supported on phenolic-resine derived active carbon and methyl iodine were used as catalyst and catalyst promoter respectively. The influences of reaction temperature, amounts of water added, space-time and amounts of carbon monoxide on the yield of carbonylation products were investigated. It was found that the reaction conditions have great effects on carbonylation. The best conditions found are following, system pressure 1.0MPa, temperature 558K, space-time of liquid 10gcat(molh-1) -1, the volume ratio of water to methanol 3:100, the molar ratio of monoxide, methanol to methyl iodine 80:40:1. Under these conditions, the yield of acetic acid is highest and can reach 67.1%, and the conversion of methanol and the yield of total carbonylized products can reach 93.8% and 79.1% respectively, which are obviously higher than the yield of product of other congener catalysts having been reported.